Environ. Sci. Technol.
1998, 32, 3094-3098
Application of Organic Amendments
To Reduce Volatile Pesticide
Emissions from Soil
J. GAN,* S. R. YATES,
S. PAPIERNIK, AND D. CROWLEY†
USDA-ARS, Soil Physics and Pesticides Research Unit,
U.S. Salinity Laboratory, 450 Big Springs Rd.,
Riverside, California 92507, and Department of Soil and
Environmental Sciences, University of California,
Riverside, California 92521
Atmospheric emission of volatile pesticides such as soil
fumigants contributes to air pollution, and feasible strategies
to reduce their emission are urgently needed. In this
study, we investigated the potential of applying organic
wastes to reduce the emission of two important fumigants,
methyl bromide (MeBr) and methyl isothiocyanate (MITC),
by enhancing their degradation in surface soil. The
degradation of both compounds was significantly accelerated
in composted manure or biosolid-manure amended soils,
and the enhancement was greater for MITC than for MeBr.
The difference in degradation kinetics between sterile
and nonsterile amended soils indicates that degradation
of MeBr in amended soils was chemically mediated, while
that of MITC was mainly a result of stimulated microbial
degradation. Applying 5% of composted manure to the 5 cm
surface soil in packed columns reduced MeBr emission
by 12%, and almost completely eliminated the volatilization
of MITC. As certain organic amendments can suppress
soil pathogens on their own, integrating fumigation
with organic waste application may potentially provide
complementary pest control activity. The applicability and
benefits of such integrations should be further evaluated
under field conditions.
Introduction
Pesticide volatilization contributes to air pollution, especially
in areas of intensive agriculture (1, 2). Of all the pesticides,
soil fumigants are potentially most volatile because of their
high vapor pressures (3). Soil fumigation is used for
controlling soilborne pathogens and parasitic nematodes,
and the practice is essential for the production of high value
crops such as strawberry and tomato, among many others.
In a recent California Air Resources Board report, the
concentrations of fumigants methyl bromide (MeBr), methyl
isothiocyanate (MITC), 1,3-dichloropropene (1,3-D), and
chloropicrin detected in the air near application sites in
California were several orders of magnitude higher than that
of the other pesticides (2). Because many fumigants have
acute and chronic toxicity, genotoxicity, or carcinogenicity,
their emissions have caused wide concern and frequently
triggered a ban of their use. In particular, emission of MeBr
from soil fumigation contributes to stratospheric ozone
* Corresponding author tel: (909) 369-4804; fax: (909) 342-4964;
e-mail: jgan@ussl.ars.usda.gov.
† University of California at Riverside.
3094 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 32, NO. 20, 1998
depletion, and a phase out in the U.S. by 2001 is currently
mandated (4). On the other hand, current agricultural
practices require fumigation as a core component of soil
pest management (5, 6). Under these circumstances,
developing approaches to minimize fumigant emission
without compromising pest control efficacy is highly desir-
able.
Volatilization of a fumigant from soil is controlled by its
rate of transport and degradation in soil. The transport of
fumigants in soil is very rapid because it is dominated by
gas-phase diffusion (7, 8). The rapid transport is evident in
that most emission loss occurs shortly after fumigation (9-
11). In contrast to the rapid transport, the degradation of
most fumigants is relatively slow, with half-lives ranging from
days to weeks (12-16). Most of the known approaches to
reduce fumigant emission, such as plastic tarping, deep
injection, surface irrigation, and packing, are based on the
suppression or delay of fumigant transport. Most of these
methods, however, have been proven to be largely ineffective
(8-10, 17-19), partly because of the slow degradation.
Conceivably, a fumigant’s emission can be reduced if its
degradation is significantly enhanced; and the negative effect
on efficacy should be potentially small if the enhanced
degradation occurs only at the soil surface.
Application of organic wastes to the soil surface is known
to stimulate soil microbial activity (20, 21), which could
potentially lead to accelerated fumigant degradation. In a
previous study, we observed that mixing 5% of a composted
manure into a sandy loam resulted in a 4-fold enhancement
of 1,3-D degradation, and incorporating 5% of the composted
manure into the top 5 cm soil layer decreased 1,3-D emissions
by 50% (16). Further, many organic wastes have been shown
to suppress soilborne pathogens by promoting disease
suppressive bacteria (20, 22-24). Thus, integration of organic
waste application with fumigation may not only reduce
fumigant emission, but also provide complementary or better
pest control. The compatibility and benefits of combining
fumigation and organic amendment, however, are essentially
untested.
The objectives of this study were to determine the effect
of two organic amendments on the degradation of MeBr and
MITC and the potential applicability for reducing their
emissions from soil. Methyl bromide is widely considered
as the most effective and difficult-to-replace fumigant (6),
and any possible extension of MeBr use beyond the proposed
phase-out date will likely depend on the availability of
techniques for reducing its emission from soil (11, 25). On
the other hand, MITC and its precursors such as metam
sodium and basimid are among the most important alterna-
tives to MeBr (6). Because of its toxicity, MITC is classified
as a Clean Air Act substance, and therefore, minimizing its
atmospheric emission is also important.
Materials and Methods
Soil, Organic Amendments, and Chemicals. The soil used
in this study, an Arlington sandy loam (coarse-loamy, mixed,
thermic, Haplic Durixeralf), was obtained from the University
of California, Riverside Agricultural Experiment Station. Fresh
soil was passed through a 2 mm sieve without air-drying and
stored at room temperature until use. The soil had a pH of
7.2 and organic matter content of 1.08%. Two different
organic amendments, a composted steer manure (CM)
purchased from a local supplier and a biosolid-manure mix
(BM) obtained from a local municipal waste treatment plant
(Recyc Inc., Corona, CA), were used. CM contained 25%
S0013-936X(98)00210-7 CCC: $15.00  1998 American Chemical Society
Published on Web 07/30/1998
carbon and 2.4% nitrogen, and BM contained 15.4% carbon
and 1.6% nitrogen.
Methyl bromide standard in a lecture bottle had a purity
of 99.5% (Aldrich, Milwaukee, WI), and MITC standard had
a purity of 99% (Sigma, St. Louis, MO). Before use, gaseous
MeBr was chilled to liquid MeBr in a sealed vial on dry ice
and stored at -15 °C. Vapam containing 45% metam sodium
was provided by Zeneca (Richmond, CA) and was used in
the column experiment.
Incubated Degradation Experiments. The first batch
incubation experiment was conducted to determine MeBr
and MITC degradation rates in soils that were amended with
the organic wastes at different ratios. The amendment ratios
(w/w) were 1:2, 1:4, 1:8, 1:20, 1:40, and 0 for CM and 1:2 and
0 for BM, where 0 served as the no-amendment control. To
prepare the amended soils, amendment and soil were
thoroughly mixed in a plastic bag, and the soil moisture was
adjusted to 18% by adding deionized water. Ten grams (oven
dried wt equivalent) of the amended soil was weighed into
21 mL headspace vials, and 5 µL of acetone solution
containing 100 µg µL-1 MeBr or MITC was added into the
soil using a microsyringe. The treated vials were immediately
capped with aluminum seals and Teflon-faced butyl rubber
septa (Supelco, Bellefonte, PA). It was found in a preliminary
experiment that the addition of 5 µL of acetone did not affect
the degradation rate of MeBr or MITC in the soil. The treated
samples were incubated at 25 ( 0.2 °C in the dark. At different
times after fumigant application, three replicated vials from
each treatment were removed and immediately stored at
-15 °C. For fumigant residue extraction, the sample vials
were opened while the soil was still frozen, and 10.0 g of
anhydrous sodium sulfate and 10.0 mL of ethyl acetate were
added to each vial, followed by immediate recapping. After
the soil was thawed at room temperature (21 °C), the vials
were mechanically shaken for 1.0 h, and an aliquot of the
solvent supernatant was transferred to a GC vial and analyzed
for fumigant concentrations on a Hewlett-Packard 5890 gas
chromatograph (GC). An electron capture detector (ECD)
was used for the detection of MeBr, and a nitrogen-
phosphorus detector (NPD) was used for the detection of
MITC. The GC conditions were 240 °C inlet temperature,
270 °C detector temperature, 1.1 mL min-1 column flow rate
(helium), RTX-624 capillary column (30 m by 0.25 mm by 1.4
µm, Restek Co., Bellefonte, CA), 35 °C isothermal column
temperature for MeBr, and 100 °C isothermal oven temper-
ature for MITC. Decline of residual fumigant concentration
in soil with time was subject to first-order fitting to obtain
the degradation rate constant k (day-1).
The second incubation experiment was conducted to
determine the mechanisms of amendment-induced fumigant
degradation. To distinguish between chemical and microbial
degradation, fumigant degradation was determined simul-
taneously in nonsterile and sterile amended soils. Sterile
amended soils were prepared by autoclaving the amended
samples twice, 1.0 h at 121 °C each time, with a 24 h interval
between the first and second autoclaving. The samples were
treated with fumigants in the same way as described above,
and the treated vials were incubated at 25 °C. Three sterilized
soils were used for each fumigant: unamended soil, soil with
CM at 1:2 (for MeBr) or 1:8 (for MITC), and soil with BM at
1:2. Residual fumigant concentrations were determined at
various times, and the kinetics of fumigant degradation was
compared between the nonsterile and sterile amended soils.
In a separate experiment, the same soil matrixes were
sterilized by adding 1000 mg kg-1 mercuric chloride (26),
and the degradation of MeBr and MITC in the sterile matrixes
was similarly followed.
Column Experiments. The effect of surface amendment
on MeBr or MITC emission losses was studied using packed
soil columns that were amended in the surface layer with or
TABLE 1. First-Order Degradation Rate Constants (k),
Half-Lives (t1/2), and Correlation Coefficients of Fitting (r2) for
Methyl Bromide Degradation in Arlington Sandy Loam Soil
Amended with Different Ratios of Organic Amendments
matrixa k (d-1) t1/2 (d) r2
soil (unamended) 0.06 ( 0.01b 12 0.93
CM-soil (1:40) 0.11 ( 0.01 6.2 0.98
CM-soil (1:20) 0.21 ( 0.01 3.30 0.99
CM-soil (1:8) 0.63 ( 0.03 1.10 0.97
CM-soil (1:4) 0.97 ( 0.02 0.71 1.00
CM-soil (1:2) 1.24 ( 0.02 0.56 1.00
BM-soil (1:2) 0.46 ( 0.05 1.50 0.90
a CM ) composted manure; BM ) Biosolid-manure mix; the ratio
following CM or BM indicates the amendment-to-soil ratio in w/w.b Mean
( standard error of k.
without CM. The columns (60 × 12.5 cm) were packed using
the Arlington sandy loam, and the initial bulk density of the
soil was 1.55 g cm-3 and the water content 0.20 cm3 cm-3.
The column system and sampling procedures are described
in detail elsewhere (27, 28). Briefly, the system consisted of
the soil column and a 5 × 12.5 cm sampling chamber that
was sealed onto the top opening of the soil column. After
the fumigant was injected into the subsoil layer through a
sampling port on the side of column, a continuous air flow
(150 mL min-1) in the sampling chamber was used to sweep
fumigant vapor above the soil surface into charcoal tubes
installed in line with the flow. Fumigant volatilization fluxes
(µg h-1) were obtained by periodically changing the sampling
tubes and analyzing fumigant residues on the GC, and the
cumulative emission loss was calculated by integrating
volatilization fluxes over the sampling durations.
Four amendment treatments were used for MeBr: (i) no-
amendment or control, (ii) 5% of CM mixed into the top 5
cm soil layer (5% CM-5 cm), (iii) 20% of CM mixed into the
top 5 cm soil layer (20% CM-5 cm), and (iv) 20% of CM mixed
into the top 10 cm soil layer (20% CM-10 cm). In MeBr-
treated columns, the soil surface was covered with poly-
ethylene film (0.0035 cm, Tri-Cal Co., Hollister, CA) to
simulate tarped fumigation. Liquid MeBr (100 µL or 173
mg) was injected into the soil 30 cm below the soil surface
using a chilled gastight syringe, and this rate was equivalent
to 140 kg ha-1. Two amendment treatments were used for
MITC: (i) no-amendment or control, and (ii) 5% of CM mixed
into the top 5 cm soil layer (5% CM-5 cm). No plastic cover
was used for the MITC treatments. Vapam (100 µL) was
injected at the 10 cm depth, and this rate was equivalent to
80 L ha-1. Duplicate columns were used for each treatment.
Fumigant volatilization was measured until the flux was no
longer detectable.
Results and Discussion
Effect of Amendment on MeBr Degradation. Degradation
of MeBr in soil was enhanced with the amendment of either
CM or BM into the soil (Table 1). At the same amendment
ratio, significantly (p < 0.001) more degradation occurred in
the CM amended soil than in the BM amended soil (Table
1). When soil was amended with CM, as the amendment
ratio increased, MeBr degradation rate also increased, and
the half-life consequently decreased. For example, the half-
life of MeBr in 1:40 CM amended soil was 6 days, but was
reduced to about 1 day or less when the amendment ratio
was 1:8 or more (Table 1). Regression analysis indicated
that the MeBr degradation rate constant k (day-1) in CM-
amended soils was linearly related to soil amendment
percentage CM% (r 2 ) 0.97):
k ) 0.068 + 0.0417 (CM%) (1)
VOL. 32, NO. 20, 1998 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 3095
FIGURE 1. Degradation of methyl bromide in sterile and nonsterile
Arlington sandy loam soil amended with different organic wastes.
Symbols are measured values, and lines are first-order regressions.
TABLE 2. First-order Degradation Rate Constants (k),
Half-Lives (t1/2), and Correlation Coefficients of Fitting (r2) for
Methyl Isothiocyanate Degradation in an Arlington Sandy
Loam Soil Amended with Different Ratios of Organic
Amendments
matrixa k (d-1) t1/2 (d) r2
soil (unamended) 0.21 ( 0.01b 3.4 0.99
CM-soil (1:40) 0.82 ( 0.03 0.8 0.99
CM-soil (1:20) 1.78 ( 0.05 0.4 0.99
CM-soil (1:8) 8.09 ( 0.56 0.1 0.95
CM-soil (1:4) 13.5 ( 1.06 0.05 0.94
CM-soil (1:2) 12.4 ( 0.36 0.06 0.99
BM-soil (1:2) 0.51 ( 0.02 1.4 0.99
a CM ) composted manure; BM ) Biosolid-manure mix; the ratio
following CM or BM indicates the ratio of amendment to soil in w/w.
b Mean ( standard error of k.
Microbial degradation of a pesticide in soil is traditionally
based on a demonstration of inhibited degradation after
sterilization. However, sterilizing amended soils resulted in
an opposite effect on MeBr degradation: MeBr degraded
faster in the sterile amended soils than in the nonsterile
amended soils (Figure 1), and the difference was significant
at the 5% level. In agricultural soils, MeBr undergoes both
chemical transformations such as hydrolysis and methylation
of organic matter (14, 15) and microbial degradation (29,
30). Methylation may occur with nucleophilic groups such
as -NH2, -NH, -SH, and -OH on the organic matter, as
illustrated from the reaction between MeBr and aniline (15).
Although not experimentally confirmed, it is likely that
autoclaving at high temperature and pressure may have
caused a structural change of the organic matter and made
the soil more reactive to MeBr, resulting in enhanced reaction
between MeBr and the soil matrix. This was confirmed when
chemical poisoning was used to sterilize the soils. In mercuric
chloride treated soils, the degradation rate of MeBr was
statistically similar to that in nonsterile soils. The effect of
sterilization on MeBr degradation, along with the linear
dependence of degradation rate on the amendment ratio,
together suggests that MeBr degradation in the amended
soils can mainly be attributed to chemical factors under the
used experimental conditions.
Effect of Amendment on MITC Degradation. In the
unamended soil, MITC had a half-life of 3.4 days (Table 2),
which is in agreement with previously reported values (12).
Compared to CM, addition of BM at the 1:2 ratio resulted in
3096 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 32, NO. 20, 1998
FIGURE 2. Degradation of methyl isothiocyanate in sterile and
nonsterile Arlington sandy loam soil amended with different organic
wastes. Symbols are measured values, and lines are first-order
regressions.
only a moderate enhancement (2.4 times) in MITC degrada-
tion, but addition of CM, even at low ratios, resulted in a
substantial increase in MITC degradation (Table 2). For
instance, at 1:40, the half-life of MITC was reduced to only
0.4 day, or the degradation was enhanced by a factor of 8.5
of that of the unamended soil. When the amendment ratio
was >1:8, the half-life was <2 h (Table 2).
Sterilizing the amended soils significantly (p < 0.001)
reduced the MITC degradation rate (Figure 2). For example,
in nonsterile soil amended at 1:8, the k value was 8.1 day-1,
but after sterilization, it was reduced to 1.5 day-1 (Table 2).
The inhibitory effect of sterilization on MITC degradation
implies that the amendment-induced MITC degradation was
primarily a result of stimulated microbial degradation. In a
previous study, it was found that microbial degradation
dominated the overall degradation of 1,3-D caused by organic
amendments (16). On the other hand, the fact that certain
amount of degradation of MITC still occurred in the sterile
amended soils suggests that chemical degradation also
contributed to the overall enhanced degradation (Figure 2).
For instance, assuming chemical and microbial transforma-
tions are additive in the same matrix, from the k values (Table
2) it can be estimated that for the 1:8 amended soil, about
20% of the overall MITC degradation would be chemical
degradation and 80% would be microbial degradation.
The mechanism for the stimulated microbial degradation
of MITC in amended soils is not known. The overall soil
respiration rate was found to increase greatly after the
addition of organic amendments (16), which implies that
the amendment may have brought into the soil a large
population of degrading organisms or nutrients that could
be used by the native soil organisms. Fumigation with MITC
has been shown to cause temporary decreases in activity
and population size of culturable heterotrophic microorgan-
isms (31), and reduced microbial activity could result in slow
fumigant degradation. The increase in biomass and mi-
crobial activity achieved by amendment addition may have
counteracted this effect, leading to rapid fumigant degrada-
tion. As shown by this research, different organic amend-
ments can have very dissimilar effects on fumigant degra-
dation, which suggests that it may also be possible to identify
compost properties (e.g., C/N ratio, microbial makeup, and
maturity) that control fumigant degradation and to use these
properties to attain a desired fumigant degradation rate.
Reduction of Fumigant Emissions by Surface Amend-
ment Application. After injection at a depth of 30 cm, MeBr
TABLE 3. Measured Total Volatilization Losses (in Percent of
Applied Chemical) of Methyl Bromide and Methyl
Isothiocyanate from Packed Soil Columns under Different
Surface Amendment Conditions (n ) 2)
treatmenta methyl bromide methyl isothiocyanate
control 68.2 ( 2.5b 21.3 ( 0.9
(no-amendment)
5% CM-5 cm 55.9 ( 0.5 0.3 ( 0.1
20% CM-5 cm 49.5 ( 2.3
20% CM-10 cm 39.6 ( 2.3
a CM ) composted manure; percent following CM indicates the
percentage of amendment in soil (w/w); the depth indicates the depth
of soil layer that was amended with CM. b Mean ( standard deviation.
rapidly diffused through the soil column and volatilized from
the soil surface. After 18 days, as much as 68% of the applied
MeBr was lost via volatilization from the unamended soil
columns (Table 3). Similar emission losses were measured
under comparable conditions in a previous study (28), and
the loss was also in agreement with recently reported field
values (9-11, 17-19). The high emission loss was apparently
caused by the rapid diffusion of MeBr through soil, the
relatively long persistence of MeBr in soil (t1/2 ) 12 days),
and the high permeability of MeBr through the polyethylene
film (3). Incorporating 5% CM into the top 5 cm soil layer
reduced MeBr emission to 55.9% (Table 3). However, the
difference between the amended and unamended treatments
only represented a limited reduction (12%). Further in-
creasing the amendment application rate resulted in further
reduced MeBr emissions (Table 3). When 20% CM was
incorporated into the top 5 cm soil layer, 49.5% of the applied
MeBr was lost by emission; when 20% of CM was mixed into
the top 10 cm soil layer, the emission loss decreased to 39.5%.
In practice, use of soil organic amendment will become
infeasible if the application rate in the top 5 cm layer is more
than 5%. Assuming that the 5 cm surface layer (bulk density
is 1.3 g cm-3) is amended, a 5% amendment application rate
will translate into approximately 30 t of material per hectare.
From the degradation experiments, the half-life of MeBr in
the soil amended with 5% CM was 3.3 days. This persistence
is apparently very long compared to the rapid diffusion. For
instance, it is estimated that during this time, as much as
61% of the total volatilization loss had already occurred.
Therefore, to achieve a greater reduction in MeBr emission,
it is necessary to further increase either the degradation rate
or the residence time of MeBr in soil. Recently, bacteria
were isolated from fumigated soil which could grow on MeBr
as a carbon source (30). Inoculation of such MeBr degrading
organisms into the amendment may be one possible avenue
for further increasing the degradation rate of MeBr under
field conditions. Using less permeable films as surface tarps
would increase the residence time of MeBr in soil, allowing
more opportunity for degradation and less emission of MeBr
(11, 25).
After the injection of Vapam at 10 cm, MITC was formed
and then gradually volatilized from soil surface, with the
maximum volatilization occurring about 2-3 days after the
application (Figure 3). Assuming 80% of the applied Vapam
was converted to MITC under the experimental conditions
(12), a total of 21.3% of the initially converted MITC was lost
by emission after 202 h (8.4 days). Adding 5% CM into the
top 5 cm soil layer, however, almost completely eliminated
MITC volatilization (Figure 3). At the end of the experiment,
a total of only 0.3% of the initially converted MITC was
emitted. The negligible emission of MITC from the amended
columns should be largely attributed to the rapid degradation
of MITC in the top soil layer that was amended with CM.
Other mechanisms, such as adsorption, should not contribute
FIGURE 3. Volatilization fluxes of methyl isothiocyanate from control
and amended soil columns after Vapam (metam sodium) was injected
at the 10 cm depth. In amended columns, 5% of a composted manure
was homogeneously mixed into the top 5 cm soil layer before
fumigant application.
significantly because previous studies showed that fumigants
are adsorbed weakly in soil (7, 12, 15).
Chemical fumigants have been used for several decades
for soilborne pest management. However, under current
practices, many of these fumigants can cause detrimental
effects to the environment when they escape into the
atmosphere. The results from our studies indicate that
common organic wastes such as composted manure are
capable of enhancing the degradation of major soil fumigants,
and the enhanced degradation may be purposely employed
to minimize fumigant emissions. Because many organic
wastes also have the ability to suppress soil pathogens, the
integration of fumigation with amendment application may
potentially offer multiple benefits. It may not only reduce
fumigant emission but also provide better pest control and,
at the same time, provide additional nutrients for plant
growth. In reality, however, as organic wastes exist in
numerous forms and their physical-chemical properties also
change greatly with origination and processing (20, 23), the
interaction of organic amendment and fumigant behavior
should be studied in a case-by-case approach. Particularly,
the effect on pest control efficacy and the effectiveness for
reducing fumigant emissions should be evaluated under field
conditions.
Acknowledgments
The authors wish to thank Q. Zhang for her assistance in
carrying out some of the experiments reported herein. This
study is supported by USDA-NRICGP Grant 22719.
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Received for review March 3, 1998. Revised manuscript re-
ceived June 10, 1998. Accepted June 29, 1998.
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